EP2054355B1 - Membrane composite de transport d'ions oxygène - Google Patents

Membrane composite de transport d'ions oxygène Download PDF

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Publication number
EP2054355B1
EP2054355B1 EP07837209A EP07837209A EP2054355B1 EP 2054355 B1 EP2054355 B1 EP 2054355B1 EP 07837209 A EP07837209 A EP 07837209A EP 07837209 A EP07837209 A EP 07837209A EP 2054355 B1 EP2054355 B1 EP 2054355B1
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Prior art keywords
layer
phase
ionic
percent
electronic
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EP07837209A
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German (de)
English (en)
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EP2054355A2 (fr
Inventor
Nagendra Nagabhushana
Jonathan Andrew Lane
Gervase Maxwell Christie
Bart Antonie Van Hassel
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Praxair Technology Inc
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Praxair Technology Inc
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    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/80—Phases present in the sintered or melt-cast ceramic products other than the main phase
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • H01M2300/0074—Ion conductive at high temperature
    • H—ELECTRICITY
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    • H01M2300/00—Electrolytes
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    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • H01M2300/0074—Ion conductive at high temperature
    • H01M2300/0077—Ion conductive at high temperature based on zirconium oxide
    • H—ELECTRICITY
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    • H01M2300/00—Electrolytes
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    • H01M2300/0094—Composites in the form of layered products, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
    • H01M4/8657—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites layered
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H01M4/9025—Oxides specially used in fuel cell operating at high temperature, e.g. SOFC
    • H—ELECTRICITY
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
    • H01M8/1253—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing zirconium oxide
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the mixture contains about 10 percent glassy carbon, 15 percent starch and a remainder of the yttrium stabilized zirconia powder. It is desirable that the oxygen transport membrane element be non-porous at the ends for sealing purposes.
  • the YSZ Powder is mixed with a binder such as PVB (Poly Vinyl Butyrl) that can be obtained from Sigma-Aldrich, 3050 Spruce Street, St. Louis, MO 63103 and then poured into an isopressing mold.
  • the isopressing mold can be a 20 mm thick flexible tube having an inner diameter of about 24.75 mm and an internal 17.75 mm diameter mandrel.

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  • Analytical Chemistry (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
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Abstract

L'invention concerne une membrane composite (1) de transport d'ions oxygène, ayant une couche dense (10), une couche de support poreuse (12), une couche poreuse intermédiaire facultative (14) située entre la couche de support poreuse (12) et la couche dense (10) et une couche d'échange de surface facultative (16), s'étendant sur la couche dense (10). La couche dense (10) possède des phases électronique et ionique. La phase ionique est composée de zircone dopée à l'oxyde de scandium, stabilisés par de l'yttrium ou du cérium. La phase électronique est composée d'un oxyde métallique contenant du lanthane, du strontium, du chrome, du manganèse et du vanadium et facultativement du cérium. La couche de support poreuse (12) est composée de zircone partiellement stabilisée par de l'yttrium, du scandium, de l'aluminium ou du cérium ou des mélanges de ceux-ci. La couche poreuse intermédiaire (14), si celle-ci est utilisée, contient les mêmes phases ionique et électronique que la couche dense. La couche d'échange de surface (16) est formée d'une phase électronique d'un oxyde métallique de lanthane et de strontium contenant également soit du manganèse soit du fer et une phase ionique de zircone dopée à l'oxyde de scandium et stabilisée par de l'yttrium ou du cérium.

Claims (10)

  1. Membrane composite de transport des ions oxygène, comprenant :
    une couche dense comportant une phase électronique et une phase ionique ;
    ladite phase électronique étant (LauSrvCe1-u-v)wCrxMnyV2O3-δ, dans laquelle u a une valeur de 0,7 à 0,9, v a une valeur de 0,1 à 0,3 et (1-u-v) est supérieur ou égal à zéro, w a une valeur de 0,94 à 1, x a une valeur de 0,67 à 0,77, y a une valeur de 0,2 à 0,3, z a une valeur de 0,015 à 0,03 et x+y+z = 1 ;
    ladite phase ionique étant Zrx'Scy'Az'O2-δ, dans laquelle y' a une valeur de 0,08 à 0,15, z' a une valeur de 0,01 à 0,03, x'+y'+z' = 1 et A représente Y ou Ce ou des mélanges de Y et de Ce ;
    une couche de support poreuse, ladite couche de support poreuse étant formée de Zrx''Ay''O2-δ, dans laquelle y'' a une valeur de 0,03 à 0,05, x''+y'" = 1, A représente Y ou Sc ou Al ou Ce ou des mélanges de Y, de Sc, de Al et de Ce.
  2. Membrane composite de transport d'ions suivant la revendication 1, comprenant en outre :
    une couche intermédiaire poreuse entre la couche dense et la couche de support poreuse ; et
    la couche intermédiaire poreuse étant constituée de la phase électronique et de la phase ionique.
  3. Membrane composite de transport d'ions suivant la revendication 2, comprenant en outre :
    une couche d'échange de surface, recouvrant la couche dense, de telle sorte que la couche dense soit située entre la couche d'échange de surface et la couche intermédiaire poreuse ;
    ladite couche d'échange de surface étant constituée d'un conducteur électronique supplémentaire formé de (Lax'''Sr1-x''')y'''MO3-δ, dans laquelle x''' a une valeur de 0,2 à 0,8, y''' a une valeur de 0,95 à 1, M = Mn, Fe et d'un autre conducteur ionique constitué de Zrx iv, ScyivAzivO2-δ. dans laquelle yiv a une valeur de 0,08 à 0,15, ziv a une valeur de 0,01 à 0,03, xiv+yiv+ziv= 1 et A = Y, Ce.
  4. Membrane composite de transport d'ions suivant la revendication 3, dans laquelle :
    la phase ionique représente 35 % à 65 % en volume de chacune des couches constituant en la couche dense et la couche poreuse intermédiaire, le reste étant constitué de la phase électronique ; et
    le conducteur ionique supplémentaire représente 35 % à 65 % en volume de la couche d'échange de surface, le reste étant constitué du conducteur électronique supplémentaire.
  5. Membrane composite de transport d'ions suivant la revendication 4, dans laquelle :
    la phase ionique représente environ 50 % en volume de chacune des couches constituant en la couche dense et la couche poreuse intermédiaire, le reste étant constitué de la phase électronique ; et
    le conducteur ionique supplémentaire représente environ 50 % en volume de la couche d'échange de surface, le reste étant constitué du conducteur électronique supplémentaire.
  6. Membrane composite de transport d'ions suivant la revendication 1, dans laquelle :
    la phase électronique est (La0,825Sr0,175)0,97Cr0,76Mn0,225V0,015O3-δ ; et la phase ionique est Zr0,89Sc0,1Y0,01O2-δ.
  7. Membrane composite de transport d'ions suivant la revendication 2, dans laquelle :
    la phase électronique est (La0,825Sr0,175)0,97Cr0,76Mn0,225V0,015O3-δ et la phase ionique est Zr0,89Sc0,1Y0,01O2-δ.
  8. Membrane composite de transport d'ions suivant la revendication 6 ou la revendication 7, dans laquelle ladite couche de support poreuse est formée de Zr0,97Y0,03O2-δ.
  9. Membrane composite de transport d'ions suivant la revendication 5, dans laquelle :
    la phase électronique est (La0,825Sr0,175) 0,97Cr0,76Mn0,225V0,015O3-δ ; la phase ionique est Zr0,89SC0,1Y0,01O2-δ ;
    ladite couche de support poreuse est formée de Zr0,97Y0,03O2-δ le conducteur ionique supplémentaire est Zr0,89SC0,1Y0,01O2-δ ; et le conducteur électronique supplémentaire est La0,8Sr0,2FeO3-δ.
  10. Membrane composite de transport d'ions suivant la revendication 9, dans laquelle :
    la couche intermédiaire poreuse a une première épaisseur comprise entre 20 micromètres et 60 micromètres, un premier diamètre moyen des pores compris entre 0,1 micromètre et 0,5 micromètre et une première porosité comprise entre 40 % et 60 % ;
    la couche intermédiaire poreuse a une deuxième épaisseur comprise entre 1 mm et 2,5 mm, un deuxième diamètre moyen des pores compris entre 2 micromètres et 5 micromètres et une deuxième porosité comprise entre 40 % et 60 % ; et
    ladite couche d'échange de surface a une troisième épaisseur comprise entre 10 micromètres et 25 micromètres, un troisième diamètre moyen des pores compris entre 0,1 micromètre et 0,5 micromètre et une troisième porosité comprise entre 40 % et 60 %.
EP07837209A 2006-08-22 2007-08-22 Membrane composite de transport d'ions oxygène Expired - Fee Related EP2054355B1 (fr)

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US11/507,486 US7556676B2 (en) 2006-08-22 2006-08-22 Composite oxygen ion transport membrane
PCT/US2007/018581 WO2008024405A2 (fr) 2006-08-22 2007-08-22 Membrane composite de transport d'ions oxygène

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CN101506122A (zh) 2009-08-12
WO2008024405A3 (fr) 2008-04-10
EP2054355A2 (fr) 2009-05-06
WO2008024405A2 (fr) 2008-02-28
BRPI0715970A2 (pt) 2013-08-06
KR20090046847A (ko) 2009-05-11
US7556676B2 (en) 2009-07-07
MX2009001959A (es) 2009-03-05
CA2660359C (fr) 2011-11-01
CN101506122B (zh) 2012-06-20
KR101395977B1 (ko) 2014-05-16
ES2379736T3 (es) 2012-05-03
US20080047431A1 (en) 2008-02-28
CA2660359A1 (fr) 2008-02-28

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